Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well...Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well designed through zeolite-imidazole framework(ZIF-67)carbonization,chemical vapor deposition,and O_(2) plasma treatment.As a result,the threedimensional NHCNBs coupled with NCNTs and unique heterojunction with rich oxygen vacancies reduce the charge transport resistance and accelerate the catalytic reaction rate of the P-Co/CoOV@NHCNB@NCNT,and they display exceedingly good electrocatalytic performance for oxygen reduction reaction(ORR,halfwave potential[EORR,1/2=0.855 V vs.reversible hydrogen electrode])and oxygen evolution reaction(OER,overpotential(η_(OER,10)=377mV@10mA cm^(−2)),which exceeds that of the commercial Pt/C+RuO_(2) and most of the formerly reported electrocatalysts.Impressively,both the aqueous and flexible foldable all-solid-state rechargeable zinc-air batteries(ZABs)assembled with the P-Co/CoOV@NHCNB@NCNT catalyst reveal a large maximum power density and outstanding long-term cycling stability.First-principles density functional theory calculations show that the formation of heterojunctions and oxygen vacancies enhances conductivity,reduces reaction energy barriers,and accelerates reaction kinetics rates.This work opens up a new avenue for the facile construction of highly active,structurally stable,and cost-effective bifunctional catalysts for ZABs.展开更多
Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability und...Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability under harsh conditions,nanodiamond has emerged as a promising carbon-based non-metallic material in the field of energy conversion such as electrocatalysis and photocatalysis.Furthermore,nanodiamond,as a new generation of green catalysts,can overcome the poisoning of catalysts by complex pollutants in advanced oxidation processes,thus effectively removing organic matter from water,which is unparalleled in reducing the cost of water purification and avoiding secondary cross-contamination of water by traditional heavy metal-based catalysts.Here,we review the research and development of nanodiamonds as major electrocatalysts and photocatalysts for energy conversion and for air/water treatment for environmental remediation.The relevant properties,trimming strategy,mechanistic understanding,and design principles of nanodiamond as a catalyst are described,as well as the challenges and prospects of this emerging field.展开更多
基金the support from the Zhejiang Provincial Natural Science Foundation (No.LR22E070001),the National Natural Science Foundation of China (Nos.12275239 and 11975205)the Guangdong Basic and Applied Basic Research Foundation (No.2020B1515120048).
文摘Herein,Co/CoO heterojunction nanoparticles(NPs)rich in oxygen vacancies embedded in mesoporous walls of nitrogen-doped hollow carbon nanoboxes coupled with nitrogen-doped carbon nanotubes(P-Co/CoOV@NHCNB@NCNT)are well designed through zeolite-imidazole framework(ZIF-67)carbonization,chemical vapor deposition,and O_(2) plasma treatment.As a result,the threedimensional NHCNBs coupled with NCNTs and unique heterojunction with rich oxygen vacancies reduce the charge transport resistance and accelerate the catalytic reaction rate of the P-Co/CoOV@NHCNB@NCNT,and they display exceedingly good electrocatalytic performance for oxygen reduction reaction(ORR,halfwave potential[EORR,1/2=0.855 V vs.reversible hydrogen electrode])and oxygen evolution reaction(OER,overpotential(η_(OER,10)=377mV@10mA cm^(−2)),which exceeds that of the commercial Pt/C+RuO_(2) and most of the formerly reported electrocatalysts.Impressively,both the aqueous and flexible foldable all-solid-state rechargeable zinc-air batteries(ZABs)assembled with the P-Co/CoOV@NHCNB@NCNT catalyst reveal a large maximum power density and outstanding long-term cycling stability.First-principles density functional theory calculations show that the formation of heterojunctions and oxygen vacancies enhances conductivity,reduces reaction energy barriers,and accelerates reaction kinetics rates.This work opens up a new avenue for the facile construction of highly active,structurally stable,and cost-effective bifunctional catalysts for ZABs.
基金funded by National Natural Science Foundation of China(Nos.52102162 and 11975205)Guangdong Basic and Applied Basic Research Foundation(Nos.2022A1515011794 and 2020B1515120048)+1 种基金the Young Talents in Higher Education of Guangdong(No.2021KQNCX273)the support from Jiangsu Science and Technology Programme-YoungScholar(BK20200251)。
文摘Benefiting from its surface-rich functional groups,eco-friendliness,impressive electrochemical properties,excellent light absorption,structural tunability at the atomic/morphological level,and ultra-high stability under harsh conditions,nanodiamond has emerged as a promising carbon-based non-metallic material in the field of energy conversion such as electrocatalysis and photocatalysis.Furthermore,nanodiamond,as a new generation of green catalysts,can overcome the poisoning of catalysts by complex pollutants in advanced oxidation processes,thus effectively removing organic matter from water,which is unparalleled in reducing the cost of water purification and avoiding secondary cross-contamination of water by traditional heavy metal-based catalysts.Here,we review the research and development of nanodiamonds as major electrocatalysts and photocatalysts for energy conversion and for air/water treatment for environmental remediation.The relevant properties,trimming strategy,mechanistic understanding,and design principles of nanodiamond as a catalyst are described,as well as the challenges and prospects of this emerging field.